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Here, cationic nanogels (NGs) are modularly engineered with tunable responsiveness, versatility, and biodegradation. Cationic PVCL\u2010based NGs with core\/shell structure are fabricated by facile one\u2010step synthesis. The formed PVCL\u2010NH<jats:sub>2<\/jats:sub> NGs exhibit uniform size, thermal\/pH dual\u2010responsive behaviors, and redox\u2010triggered degradation. Moreover, the NGs can be employed to modify or\/and load with various functional agents to construct multipurpose nanoplatforms in a modular manner. Notably, the novel hybrid structure with copper sulfide (CuS) NPs loaded in the NGs shell is prepared, which leads to higher photothermal conversion efficiency (31.1%) than other CuS randomly loaded NGs reported. By personalized tailoring, these functionalized NGs display fluorescent property, <jats:italic>r<\/jats:italic><jats:sub>1<\/jats:sub> relaxivity, strong near\u2010infrared (NIR) absorption, good biocompatibility, and targeting specificity. The superior photothermal effect of hybrid NGs (CuS@NGs\u2010LA) is presented under NIR II over NIR I. Importantly, hybrid NGs encapsulated doxorubicin (CuS@NGs\u2010LA\/DOX) show endogenous pH\/redox and exogenous NIR multi\u2010triggered drug release for efficient photothermal\u2010chemotherapy, which can completely eliminate advanced tumors and effectively inhibit recurrence. Overall, the pervasive nanoplatforms based on intelligent cationic NGs with tunable responsiveness, versatility, and biodegradation are developed by engineered modular strategy for precision medicine applications.<\/jats:p>","DOI":"10.1002\/adfm.202100227","type":"journal-article","created":{"date-parts":[[2021,3,24]],"date-time":"2021-03-24T02:48:20Z","timestamp":1616554100000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":144,"title":["Multi\u2010Responsive Biodegradable Cationic Nanogels for Highly Efficient Treatment of Tumors"],"prefix":"10.1002","volume":"31","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-7837-7874","authenticated-orcid":false,"given":"Xin","family":"Li","sequence":"first","affiliation":[{"name":"DWI\u2010Leibniz\u2010Institute for Interactive Materials e.V.  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Forckenbeckstr. 50 52056 Aachen Germany"},{"name":"Institute for Technical and Macromolecular Chemistry RWTH Aachen University  Worringerweg 2 52074 Aachen Germany"}]},{"given":"Yu","family":"Luo","sequence":"additional","affiliation":[{"name":"School of Chemical Science and Engineering Tongji University  1239 Siping Road Shanghai 200092 P. R. China"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-6785-6645","authenticated-orcid":false,"given":"Xiangyang","family":"Shi","sequence":"additional","affiliation":[{"name":"College of Chemistry Chemical Engineering and Biotechnology Donghua University  2999 North Renmin Road Shanghai 201620 P. R. 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